Journal
CHEMISTRY-A EUROPEAN JOURNAL
Volume 25, Issue 50, Pages 11670-11679Publisher
WILEY-V C H VERLAG GMBH
DOI: 10.1002/chem.201901806
Keywords
carbon dioxide; cryptates; methane; photoreduction; visible light
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Funding
- Fundacao para a Ciencia e a Tecnologia, Portugal [UID/MULTI/00612/2019, UID/MULTI/04046/2019, PTDC/QEQQIN/3414/2014]
- FCT [SFRH/BPD/73345/2010, PD/BD/52368/2013]
- FTC [CEECIND/00509/2017]
- Fundação para a Ciência e a Tecnologia [SFRH/BPD/73345/2010, PD/BD/52368/2013] Funding Source: FCT
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Three Co-II octaazacryptates, with different substituents on the aromatic rings (Br, NO2, CCH), were synthesised and characterised. These and the already published non-substituted cryptate catalysed CO2 photoreduction to CO and CH4 under blue visible light at room temperature. Although CO was observed after short irradiation times and a large range of catalyst concentrations, CH4 was only observed after longer irradiation periods, such as 30 h, but with a small catalyst concentration (25 nm). Experiments with C-13 labelled CO2 showed that CO is formed and reacts further when the reaction time is long. The CCH catalyst is deactivated faster than the others and the more efficient catalyst for CH4 production is the one with Br. This reactivity trend was explained by an energy decomposition analysis based on DFT calculations.
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